Widespread use of magnetic resonance spectroscopic imaging techniques is hindered by several challenges, including low signal-to-noise ratio (SNR), inhomogeneity of the main field and RF excitation field, cumbersome constraints on imaging time and volumetric coverage, and limited ability to detect and separate signals from coupled or overlapping spectral components. We address these limitations by developing spectroscopic acquisition and processing methods for i) high field strength (3T and 7T), providing higher SNR, increased chemical shift dispersion and simplified coupling patterns;ii) spiral readout gradients that address the spatial encoding limitations in MRSI by offering two orders of magnitude of encoding acceleration;iii) parallel RF transmission to mitigate the severe non-uniformity of RF excitation at high field;and iv) receive coil arrays to improve SNR and enable parallel encoding. Several attractive spectroscopic imaging applications provide a strong motivation for this work, including volumetric, high spatial resolution spectroscopic imaging, greatly reduced scan times for improved patient tolerance, and the incorporation of multidimensional methods to detect subtly different chemical shift species.